The removal of heavy metals from aqueous solution using ...
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ORIGINAL ARTICLE
The removal of heavy metals from aqueous solution using naturalJordanian zeolite
Yazan Taamneh1 • Suhail Sharadqah2
Received: 27 November 2015 / Accepted: 14 January 2016 / Published online: 2 February 2016
� The Author(s) 2016. This article is published with open access at Springerlink.com
Abstract In this article, the adsorption process of cad-
mium and copper using natural Jordanian (NJ) zeolite as
adsorbent has been experimentally estimated. The samples
of NJ zeolite were obtained from Al Mafraq discrete, north
east of Jordan. The influence of the bulk concentration
(Co), contact time (t) and different adsorbent masses (m) of
NJ zeolite on the removal of heavy metal were evaluated.
These variables had a considerable function in promoting
the sorption process of heavy metal using the NJ zeolite.
The initial concentration of heavy metals in the stock
solution was extended between 80 and 600 mg/L. The
batch adsorption method was employed to investigate the
adsorption process. The experimental data were correlated
using Freundlich and Langmuir empirical formula. The
ability of NJ zeolite to eliminate cadmium and copper was
estimated according to Langmuir isotherm empirical for-
mula and found 25.9 and 14.3 mg/g for cadmium and
copper, respectively. The kinetics of adsorption of cad-
mium and copper have been analyzed and correlated by
first-order and second-order reaction model. It was noticed
that adsorption of cadmium and copper was better corre-
lated with pseudo-second-order kinetic model. The results
presented that NJ zeolite is practical adsorbent for
removing cadmium and copper ion metal.
Keywords NJ zeolite � Batch process � Cadmium �Copper � Isotherm � Kinetic
Introduction
The major industrial sources impact the environment as a
result of producing heavy metals. The existence of heavy
metals in wastewater due to many manufacturing processes
is a legalized problem worldwide. The most common
sources of heavy metals obtained from surface finishing
processes as well as industrial products that ends up in
wastewater (Hui et al. 2005; Karvelas et al. 2003; Ahlu-
walia 2007). Removing heavy metals from industrial
wastewater required high energy or special operational
requirements. Several techniques such as adsorption,
extraction, disambiguation, clotting, ion-exchange, and
membrane processes are supposed for the handling of
wastewater pollution (Babel and Kurniawan 2003a; Wang
and Peng 2010a; Kwon et al. 2010). Adsorption method
form an appropriate method for wastewater handling
because of its cost effectiveness and simplicity, among all
these methods (Gupta et al. 2006; Ali 2012; Yadanaparthi
et al. 2009; Argun 2008; Rashed 2011).
Regardless of the effectiveness of activated carbon for
prevailing the metal ions load, particular attention have
been drawn by several inspector to the common adsorbents
like silica, sand, activated alumina, clays, and natural
zeolite for their relatively low costs and natural charac-
teristics (Panayotova 2001; Bailey et al. 1999; Babel and
Kurniawan 2003b). Actually, zeolite gains progressive
attraction of many investigator because of its special
characteristic such as ion exchange capacity, hydration-
dehydration, and adsorption (Caputo and Pepe 2007; Wang
and Peng 2010b; Zhang 2006).
& Yazan Taamneh
1 Department of Aeronautical Engineering, Jordan University
of Science and Technology, P.O. Box 3030, Irbid 22110,
Jordan
2 Department of Natural Resources and Chemical Engineering,
Tafila Technical University, P.O. Box 179, Tafila 66110,
Jordan
123
Appl Water Sci (2017) 7:2021–2028
DOI 10.1007/s13201-016-0382-7
Zeolites are aluminosilicate minerals of alkali or alka-
line earth metal which contains crystal water. Zeolites
consist of three-dimensional networks of aluminate and
silicone dioxide tetrahedral linked by partnership of all
oxygen atoms. The voids make up from 20 to 50 % of the
total crystal volume of most zeolites. (Mumpton 1978,
1996; Gottardi 1978). For wastewater treatment, the most
important properties of natural zeolite are cation exchange
capacity and ion selectivity (Colella 1996).
Removing of heavy metal by natural zeolites with
respect to Co2?, Cu2?, Zn2?, and Mn2? were studied by
Erdem et al. (2004). The study achieved using batch pro-
cess technique and the effect of varying the initial heavy
metal concentration also considered. They concluded that
the adsorption process rely on bulk density and size of
hydrated ion. The selectivity succession of metal ionic
according to their equilibrium studies was specified like
Co2?[Cu2?[Zn2?[Mn2?.
Loizidou and Townsend (1987) indicated that natural
zeolite is able to eliminate some of heavy metals effec-
tively from industrial wastewater. The ability of the zeolite
to be regenerated is an important issue that must be well
considered together with the other relevant properties such
as its selectivity to eliminate heavy metals toxicity from
aqueous solutions.
There are a large number of processes that have been
improved and used over the years to eliminate dissolved of
cadmium and copper in industrial wastewater treatment
using clotting, adsorption, ion exchange, extraction, etc.
(Lewinsky 2006; Blocher et al. 2003; Izanloo and Nasseri
2005; Dhaba and Hussein 2014). This conventional tech-
nique is often neither effective nor economically especially
when the cadmium and copper ion metal are presented at
relatively low concentration.
Recently, Rao et al. (2005) evaluated the sorption pro-
cess for cadmium and copper from aqueous solutions using
activated coal. The effect of initial heavy metal load,
adsorbent mass, and time contacting on adsorption ability
were estimated. They analyzed and correlated the experi-
mental data according to both Freundlich and Langmuir
model. The highest uptake of copper and cadmium was
found to be 20 mg/g for cadmium and copper. The maxi-
mum uptake capacities of cadmium and copper were 88
and 90 %, respectively.
Zeolite was reported for the first time in Jebel Aritain
discrete (Jordan) in 1987. Since that, various studies have
been carried out to inspect the genesis applicability of NJ
zeolites in different applications such as, water treatment,
agriculture, water filter and the environmental protection
(Dwiri 1987; Sharadqah and Al-Dwairi 2010).
The capability of Jordanian zeolite was studied by
Marashdeh et al. (2009), to eliminate heavy metals (Cr and
Cd from electroplating wastewater). Batch and continues
packed column experiments were used for sorption of
metal in their single and binary solution. The bulk con-
centration of Cd2? and Cr3? ranged from 50 to 75 mg/L.
The experimental results showed that the uptake capacities
increase with initial heavy metal concentration. From the
equilibrium studies the adsorption capacity of zeolite for
cadmium qe = 25.5 mg/g was higher than that for chrome
qe = 19.75 mg/g. The uptake of both metals was decreased
when combined together with equal concentration in a
solution, 64 % decrease for cadmium qe = 9.5 mg/g and
31 % decrease for chromium qe = 13.5 mg/g.
A packed bed column was constructed by Taamneh and
Dwairi (2013) to estimate the capacity of NJ zeolite to
bring out nickel from aqueous solutions. The NJ zeolite
specimen was picked up from Jabal AL Aritayn discrete
(Jordan). The experimental results of adsorption process in
a packed bed column are used to bear out the accuracy of
Klinkenberg correlation model. The Klinkenberg equation
was employed to predict the effective diffusivity constant.
Baker et al. (2009) investigated the uptake capacity of heavy
metals ions likeCr3?, Cd2?, Cu2?, andPb2?usingNJzeolite for
batch and packed bed column at the following condition:
pH 3.0, volume of solution 1 L, temperature of 25 �C and
phillipsite dose5 g.The Jordanianphillipsite tuff presentedhigh
selectivity for the discharge of lead about 98 % achievedwithin
90 min, then chrome (III), copper, and cadmium about 96 %
removal achieved within 5 h. The adsorption capacity of
phillipsite tuff by assuming initial concentration of cadmium
30 mg/L was calculated about 0.24 mg Cd/g zeolite.
As concluded from literature review, NJ zeolites have
been used to eliminate different heavy metals ions from
prepared synthetic solution. But there has been no effort
devoted to correlate the experimental data with both
sorption isotherm and kinetics model. In this work, our aim
object is to investigate the adsorption process of cadmium
and copper on NJ zeolite and correlate the data with well-
known isotherms and kinetic model.
Materials and methods
Natural Jordanian zeolite (NJ zeolite)
The samples of natural zeolite were picked up from Al-
Mafraq area, northeast of Jordan. The bulk sample was
washed by distilled water to eliminate most of the surface
dust. Then the sample was crushed and sieved into two
different grain sizes (less than 0.4 mm and 0.4–4 mm). The
experiments were performed with grain size distribution
less than 0.4 mm in diameter. Their distribution was
measured using laser diffraction instrument (see Fig. 1).
2022 Appl Water Sci (2017) 7:2021–2028
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X-ray diffraction was obtained before and after treatment
with sodium chloride. The chemical analyses composition
of NJ zeolite was given by Taamneh and Dwairi (2013).
Chemicals and adsorption studies
Cadmium and copper nitrate which have been diluted in
distilled water are used throughout the experiments. The
chemicals and reagent were supplied from Merck (Ger-
many) and of analytical grade using deionized water. The
concentrations of cadmium and copper solutions were
varied from 100 to 600 mg/L by diluting the stock solution.
The ion exchange process on NJ zeolite was accomplished
using the batch method. Throughout all the experiments,
the pH value was adjusted and kept constant using 0.1 N
NaOH. The glass bottles were then put on shaker for 24 h
to attain the equilibrium. 5 g of NJ zeolite was used in the
batch adsorption experiments with 250 mL of solutions
containing different heavy metal concentration at constant
pH. To have relatively clean samples for atomic absorption
spectrometer analyses, filter paper (Whatman No. 43) was
used. The concentration of metal ions in initial and final
solution was measured by Atomic Absorption Spectrome-
ter (AAS). The effects of concentration (100–600 mg/L),
adsorption dose (5–80 g) and contact time (1–60 min) were
estimated.
Sorption isotherm models
In this work, the batch adsorption technique was selected to
study the adsorption and kinetic models for cadmium and
copper uptake. The adsorption experimental results of
cadmium and copper on NJ zeolite were analyzed
according to well-known isotherm model (Freundlich and
Langmuir). The uptake of heavy metal through a sequence
of batch test was calculated using the following equation:
(a) (b)
(c)
0
20
40
60
80
100
0
0,1
0,2
0,3
0,4
0,5
0,6
0 500 1000 1500
Q3q3
X(µm)
(d)
Fig. 1 a Crystallization, b pores shape, c particle size distribution, d raw materials of NJ zeolite
Appl Water Sci (2017) 7:2021–2028 2023
123
qe ¼Co � Ce
m=Vð1Þ
where qe is the weight of heavy metal uptake per unit of NJ
zeolite (mg/g); Co and Ce are the initial and equilibrium
concentration in the samples (mg/L), respectively; m is the
adsorbent mass (mg) and V is the aqueous volume (L).
Kinetic studies
The sorption kinetic results of cadmium and copper on the
NJ zeolite were analyzed according to first and second
sorption kinetic equation (Sevil and Bilge 2007). Samples
were sucked from the glass bottle every 2 min using glass
syringe. The remaining of cadmium and copper concen-
tration in the solution was also analyzed by AAS (atomic
absorption spectrophotometer).
Results and discussion
Effect of metal concentration
To find the optimum concentration, experimental studies
were carried out for a wide range of metal concentrations
between 100 and 600 mg/L. The capability of sorption
process was found to be stable and reached a maximum
value at concentration 100 mg/L. This is because the surface
where the adsorption occurs reaches its maximum uptake,
i.e. no more metal ions can be adsorbed. It is also clear from
Fig. 2 that the percentage of Cd and Cu removal decreases
by increasing initial metal concentration. This result pointed
out that with increasing metal concentration less favorable
spaces become involved in the aqueous solution.
In this study the metal ion uptake could be referred to
ion-exchange kinetics in the micro porous of NJ zeolite.
Metal ions had to move through the pores of the zeolite
mass as well as through channels of the lattice during the
ion-exchange process and they had to substitute their
cations. The adsorption percentage was larger for cadmium
compared with copper.
Effect of NJ zeolite volume
The effect of NJ zeolite load on the uptake efficiency of
cadmium and copper is presented in Fig. 3. The amount of
zeolite required for quantitative removal of cadmium and
copper from an initial metal concentration 7 mg/L was
found to be 30 mg.
The adsorption percentage increased with zeolite mass
in case of both cadmium and copper and when the adsor-
bent reaches beyond 30 mg became steady. The adsorption
percentage was found to be 46, 15.5 % in the case of
cadmium and copper, respectively, for identical zeolite
dose (1 mg). It is clear that the uptake efficiency of cad-
mium and copper increases with the concentration of NJ
zeolite. The reason for this may be the surface area of the
zeolite at higher mass concentration of zeolite is more
available. Therefore, the heavy metal ions have the possi-
bility to exchange their sites over a large available surface
area.
Effect of contact time
The effect of contact time on adsorption efficiency is
depicted in Fig. 4. It is clear from Fig. 4 that the contact
time needed to reach the maximum removal of metal by NJ
zeolite was dependent on the type of heavy metal. From the
economic system point of view, the role of the equilibrium
time assessment is very important especially in many
wastewater treatment applications. The equilibrium
adsorption was attained through 20 min for both cadmium
0
0,1
0,2
0,3
0,4
0,5
0,6
0,7
0,8
0,9
1
0 100 200 300 400 500 600 700
Ads
orpt
ion
%
Co (mg/l)
Cd
Cu
Fig. 2 Removal efficiency of heavy metal (Cd and Cu) on NJ zeolite.
mz = 5 g, V = 250 ml, pH 6, time 24 h
Fig. 3 Heavy metal removal (Cd and Cu) as a function adsorbent
dose (NJ zeolite). Co = 7 mg/L, V = 25 mL, pH 6, time 24 h
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and copper metal and the equilibrium adsorption were
determined at 80 and 68 mg/g (Fig. 4).
Adsorption isotherms
Freundlich empirical equation
Although the model was first proposed extensively as an
empirical equation by Freundlich (1932), many other
researchers used it. Currently, Freundlich model is used in
organic compounds or high-selectivity species on activated
charcoal and molecular sieves. Freundlich empirical can be
given by:
qe ¼ kFC1=ne ð2Þ
The parameters kF and 1/n are Freundlich constant and
sorption intensity, respectively, and these two parameters
are dependent on temperature. By taking the natural
logarithm of both side of Eq. 2 we get:
log qe ¼ log kF þ1
nlogCe ð3Þ
The two parameters of Freundlich model can be
calculated for cadmium and copper from the slope and
intercept of the linear plot (see Table 1). The experimental
data are fitted according to the linear form of Eq. (2).
qe ¼ 20C5:25e r2 ¼ 0:98 for Cd ð4Þ
qe ¼ 11C4:4e r2 ¼ 0:96 for Cu ð5Þ
Langmuir equation
Langmuir models primarily developed to demonstrate gas–
solid phase adsorption onto activated charcoal and it has
conventionally been used to assess the performance of
different adsorption systems including solid liquid systems.
Langmuir model supposes monolayer adsorption, i.e. all
the adsorbed molecules are in contact with the surface layer
of the adsorbent. This model is presented by:
qe ¼QmkCe
1þ kCe
ð6Þ
where qe and Ce are the equilibrium concentration of
cadmium or copper in the JN zeolite and aqueous solution
in mg/g and mg/L, respectively, Qm is the sorption
capacity, k is the energy of sorption constant. The linear
form of Langmuir isotherm equation is given by:
Ce
qe¼ 1
kQm
þ Ce
Qm
ð7Þ
The Langmuir isotherm linear equation for cadmium
and copper adsorption on NJ zeolite is given by:
Ce
qe¼ 0:00421þ 0:04Ce r2 ¼ 0:98 for Cd ð8Þ
Ce
qe¼ 0:0095þ 0:0699Ce r2 ¼ 0:97 for Cu ð9Þ
The Freundlich and Langmuir isotherm parameters
and the statistical fits of cadmium and copper adsorption
using NJ Zeolite are presented in Table 1. It is very
important to analyze the experimental data in terms of
Langmuir and Freundlich isotherm sorption models. The
sorption constant and regression coefficient for both
Freundlich and Langmuir sorption model are given in
Table 1. The comparison between the experimental
adsorption results with the empirical isotherm models
(Freundlich and Langmuir model) on cadmium and
copper using NJ zeolite sorbent are depicted in Fig. 5. It
can be noted from Fig. 5 that the adsorption
experimental results are better fitted to Freundlich
isotherm model than to Langmuir isotherm model. The
calculated sorption capacities for cadmium and copper
fitted to Langmuir linear equation were 25.9 and
14.3 mg/g, respectively. The parameters kF and n were
calculated by linear Freundlich equation from
experimental sorption data as 20, 5.2 for cadmium and
11, 4.4 for copper (see Table 1).
Fig. 4 Variation of heavy metal removal (Cd, Cu) on NJ zeolite as
function of contact time: Co = 7 mg/L, V = 25 ml, pH 6, time 24 h
Table 1 Freundlich and Langmuir constant
Cadmium Copper
Freundlich isotherm constant
KF 20 11
n 5.2 4.4
r2 0.98 0.97
Langmuir isotherm constant
Qm 25.9 14.3
k 9.5 7.36
r2 0.97 0.98
Appl Water Sci (2017) 7:2021–2028 2025
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Sorption kinetic models
The amount of cadmium and copper adsorbed, qt, at time t
was calculated from the following equation:
qt ¼Co � Ce
m=Vð10Þ
The removal of copper and cadmium from zeolite as a
function of time can be mathematically expressed in terms
of different kinetic adsorption models such as:
Pseudo-first-order kinetic model (Langerhans rate
equation)
Pseudo-first-order kinetic model supposes that the rate of
change of adsorbate uptake with time is directly propor-
tional to the difference in the equilibrium concentration and
the amount of adsorbate uptake with time (Ho and McKay
1998). The kinetic rate in differential form Eq. (11) and
after integration Eq. (12) is obtained:
dqt
dt¼ k1ðqe � qtÞ ð11Þ
lnðqe � qtÞ ¼ �k1t þ ln qe ð12Þ
Pesudo-second-order kinetic model
In this model (Ho et al. 1996), the kinetic rate in differ-
ential form and it is analytical solution can be expressed as
dqt
dt¼ k2ðqe � qtÞ2 ð13Þ
t
qt¼ 1
k2q2eþ t
qeð14Þ
To estimate the adsorption rate constant of cadmium and
copper, the first-order model was used. The rate constant
(k1) for cadmium and copper adsorption onto NJ zeolite
were 0.5145, 0.325, respectively. Meanwhile the second-
order reaction rate constant (k2) for cadmium and copper
adsorption onto NJ zeolite were 2.32145, 1.716,
respectively.
The time dependency of removal rate of cadmium and
copper on NJ zeolite are shown in Fig. 6. The kinetic rate
study of cadmium and copper on NJ zeolite was carried out
with different time, at room temperature 22� C, constantmetal concentration 250 mg/L, 80 g of NJ zeolite and
pH 6. The value of the first and second reaction rate con-
stant (k1, k2) obtained from sorption kinetic models are
used to correlate experimental data on NJ zeolite. It can be
noted that the second reaction constant has higher value for
the sorption kinetic of cadmium and copper on NJ zeolite.
It is clear from values of second-order constant that cad-
mium and copper sorption onto the NJ zeolite follows the
second-order model. Thus, rate of sorption according to the
second-order model for cadmium and copper are faster
than first-order model. For example, the cadmium uptake
capacities were completed within 10 min. Meanwhile, the
copper uptake capacity completed within 20 min. Figure 6
shows that cadmium metal has higher uptake capacity than
copper. As a result of sorption kinetic, the second-order
model can demonstrate the sorption process and very well
correlated with the experimental results. Therefore, the
second-order equation is valuable for the kinetic sorption
studied in this work.
Conclusion
The adsorption capacity of cadmium and copper using NJ
zeolite has been experimentally investigated. It was con-
cluded that metal bulk concentration, adsorption time and
mass of adsorbent, are an important factors that affect the
Fig. 5 Adsorption isotherms experimental data of cadmium and
copper on NJ zeolite compared with Freundlich and Langmuir
isotherm model at the same condition
0
0,2
0,4
0,6
0,8
1
0 10 20 30 40 50 60 70
q t(m
g/g)
t/min
Cd
Cu
Pseudo 2nd order
Pseudo 1st order
Fig. 6 Sorption kinetic experimental data of cadmium and copper on
NJ zeolite compared with first- and second-order model at the same
condition
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123
adsorption process. These parameters had a considerable
trace on the uptake of cadmium and copper metal using NJ
zeolite. A widely used isotherm and kinetic models to
present study to estimate the equation parameters were
employed.
The Freundlich and Langmuir isotherms models are
used to describe the experimental adsorption results
meanwhile the pseudo-first- and second-order kinetics
model are used for kinetic rate elaboration. It was set that
the Freundlich empirical is well demonstrated and fitting
the experimental results. The metal ion uptake capacities
for cadmium and copper were 25.9 and 14.3 mg/g,
respectively. The calculated adsorption intensity parameter
correlated to Langmuir isotherm model for cadmium and
copper are 9.5 and 7.36, respectively. Cadmium and copper
adsorption from aqueous solution using NJ zeolite was well
demonstrated with the second-order kinetic model. The
experimental adsorption data were better adequate to the
second-order model than to the first-order model. As a
result of this study, the NJ zeolite for the removal of
cadmium and copper using a batch adsorption technique
has inherent advantages.
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